The effect of heat treatment on the performance and structure of carbon-supported Au-Pd catalysts for the direct synthesis of hydrogen peroxide

被引:99
作者
Edwards, Jennifer K. [1 ]
Pritchard, James [1 ]
Piccinini, Marco [1 ]
Shaw, Greg [1 ]
He, Qian [2 ]
Carley, Albert F. [1 ]
Kiely, Christopher J. [2 ]
Hutchings, Graham J. [1 ]
机构
[1] Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Cardiff CF10 3AT, S Glam, Wales
[2] Lehigh Univ, Dept Mat Sci & Engn, Bethlehem, PA 18015 USA
基金
英国工程与自然科学研究理事会;
关键词
Gold palladium nanoparticles; Hydrogen peroxide direct synthesis; Aberration-corrected microscopy; ACTIVATED CARBON; H2SO4/ETHANOL SYSTEM; PALLADIUM CATALYSTS; PD/SIO2; CATALYST; LIQUID-PHASE; H-2; O-2; H2O2; ACID; OXIDATION;
D O I
10.1016/j.jcat.2012.05.018
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The direct synthesis of hydrogen peroxide using supported gold palladium catalysts prepared by incipient wetness impregnation is described and discussed. The effect of an acid pre-treatment step on the activated carbon support prior to the deposition of the metals, together with the effect of the calcination temperature, has been investigated. The acid pre-treated samples all show superior activity to those materials prepared with the omission of this acid pre-treatment stage. The calcination temperature affects both the re-usability and hydrogenation activity of the catalysts. Detailed characterisation using X-ray photoelectron spectroscopy and aberration-corrected scanning transmission electron microscopy is described. The enhanced activity is associated with a higher surface concentration of palladium in the acid pre-treated samples which is principally present as Pd2+. Calcination of the catalysts at 400 degrees C is required to achieve re-usable and stable catalysts, and this is associated with the morphology and dispersion of the metal nanoparticles. The surface ratio of Pd-0/Pd2+ is found to be an important factor controlling the hydrogenation of hydrogen peroxide, and a series of controlled reduction and re-oxidation of a sample show how the Pd-0/Pd2+ surface ratio can influence the relative rates of hydrogen peroxide synthesis and hydrogenation. (C) 2012 Elsevier Inc. All rights reserved.
引用
收藏
页码:227 / 238
页数:12
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